FeII, CoII and NiII complexes of two tetraazamacrocycles (1,4,8,11-tetrakis(carbamoylmethyl)-1,4,8,11-tetraazacyclotetradecane (L1) and 1,4,7,10-tetrakis(carbamoylmethyl)-1,4,7,10-tetraazacyclododecane (L2) show promise as paraCEST agents for registration of temperature (paraCEST = paramagnetic Chemical Exchange Saturation Transfer). The FeII, CoII and NiII complexes of L1 show up to four CEST peaks shifted ≤ 112 ppm, whereas analogous complexes of L2 show only a single CEST peak at ≤ 69 ppm. Comparison of the temperature coefficients (CT) of the CEST peaks of [Co(L2)]2+, [Fe(L2)]2+, [Ni(L1)]2+ and [Co(L1)]2+ showed that a CEST peak of [Co(L1)]2+ gave the largest CT (−0.66 ppm/°C at 4.7 T). NMR spectral and CEST properties of these complexes correspond to coordination complex symmetry as shown by structural data. The [Ni(L1)]2+ and [Co(L1)]2+ complexes have a six-coordinate metal ion bound to the 1-, 4- amide oxygens and four nitrogens of the tetraazamacrocycle. The [Fe(L2)]2+ complex has an unusual eight-coordinate FeII bound to four amide oxygens and four macrocyclic nitrogens. For [Co(L2)]2+, one structure has seven-coordinate CoII with three bound amide pendents and a second structure has a six-coordinate CoII with two bound amide pendents.